Judul Artikel : Cigarette Butt Waste as Material for Phase Inverted

Membrane Fabrication Used for Oil/Water Emulsion

Separation

Penulis : Aris Doyan, Chew Lee Long, Muhammad Roil Bilad, Kiki

Adi Kurnia, Susilawati, Saiful Prayogi, Thanitporn

Narkkun, dan Kajornsak Faungnawakij

Nama Jurnal : Polymers

Penyelenggara/Penerbit : Multidisciplinary Digital Publishing Institute (MDPI)

Halaman : 1-15

Volume : 13

Web Jurnal : https://www.mdpi.com/2073-4360/13/12/1907

URL Dokumen : https://www.mdpi.com/2073-4360/13/12/1907/html

DOI : https://doi.org/10.3390/polym13121907

Tanggal/Waktu : Juni 2021

Satuan : 12 Issue/Tahun

Volume Kegiatan : 1

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CERTIFICATE OF PUBLICATION

Certificate of publication for the article titled:

Cigarette Butt Waste as Material for Phase Inverted Membrane Fabrication Used forOil/Water Emulsion Separation

Authored by:

Aris Doyan; Chew Lee Leong; Muhammad Roil Bilad; Kiki Adi Kurnia; Susilawati Susilawati;Saiful Prayogi;

Thanitporn Narkkun; Kajornsak Faungnawakij

Published in:

Polymers 20212021, Volume 13, Issue 12, 1907

an Open Access Journal by MDPI

IMPACTIMPACTFACTORFACTOR3.4263.426

CITESCORECITESCORE

4.74.7 SCOPUSSCOPUS

Basel, June 2021

an Open Access Journal by MDPI

Cigarette Butt Waste as Material for Phase Inverted MembraneCigarette Butt Waste as Material for Phase Inverted MembraneFabrication Used for Oil/Water Emulsion SeparationFabrication Used for Oil/Water Emulsion Separation

Aris Doyan; Chew Lee Leong; Muhammad Roil Bilad; Kiki Adi Kurnia; Susilawati Susilawati;Saiful Prayogi; Thanitporn Narkkun; Kajornsak Faungnawakij

Polymers 20212021, Volume 13, Issue 12, 1907

Polymers 2021, 13, x. https://doi.org/10.3390/xxxxx www.mdpi.com/journal/polymers

Article 1

Cigarette Butt Waste as Material for Phase Inverted Membrane 2

Fabrication Used for Oil/Water Emulsion Separation 3

Aris Doyan 1,2,*, Chew Lee Leong 3, Muhammad Roil Bilad 3,4,*, Kiki Adi Kurnia5, Susilawati Susilawati 1,2, Saiful 4

Prayogi 4, Thanitporn Narkkun 6 and Kajornsak Faungnawakij 6 5

1 Master of Science Education Program, University of Mataram, Jl. Majapahit No. 62 Mataram 83125, 6 Indonesia; aris_doyan@unram.ac.id (A.D.); susilawatihambali@unram.ac.id (S.S) 7

2 Physics Education, FKIP, University of Mataram, Jl. Majapahit No. 62 Mataram 83125, Indonesia 8 3 Department of Chemical Engineering, Universiti Teknologi PETRONAS, Bandar Seri Iskandar 32610, Perak, 9

Malaysia; leongchewlee@gmail.com (C.L.L.) 10 4 Faculty of Applied Science and Technology, Universitas Pendidikan Mandalika (UNDIKMA), Jl. Pemuda 11

No. 59A, Mataram 83126, Indonesia; muhammadoilbilad@ikipmataram.ac.id (M.R.B.); 12 saifulprayogi@ikipmataram.ac.id (S.P.) 13

5 Department of Marine, Faculty of Fisheries and Marine, Universitas Airlangga, Kampus C Jalan Mulyorejo, 14 Surabaya 60115, Indonesia; kiki.adi@fpk.unair.ac.id (K.A.K.) 15

6 National Nanotechnology Center (NANOTEC), National Science and Technology Development Agency 16 (NSTDA), 111 Thailand Science Park, Pathum Thani 12120, Thailand; thanitporn.nar@ncr.nstda.or.th (T.N.); 17 kajornsak@nanotec.or.th (K.F.) 18

19 * Correspondence: aris_doyan@unram.ac.id (A.D.) and muhammadoilbilad@ikipmataram.ac.id (M.R.B.) 20

Abstract: The increasing rate of oil and gas production has contributed to a release of oil-in-water 21

emulsion or mixtures to the environment, becoming a pressing issue. At the same time, pollution of 22

the toxic cigarette butt has also become a growing concern. This study explored utilization of 23

cigarette butt waste as a source of cellulose acetate-based (CA) polymer to develop phase inverted 24

membrane for treatment of oil/water emulsion and compared with commercial polyvinylidene 25

difluoride (PVDF) and polysulfone (PSF). Results show that CA-based membrane from waste 26

cigarette butt offers an eco-friendly material without compromising the separation efficiency, with 27

a pore size range suitable for oil/water emulsion filtration with the rejection of >94.0%. The CA 28

membrane poses good structural property like established PVDF and PSF membranes with equally 29

asymmetric morphology. It also poses hydrophilicity properties with a contact angle of 74.5°, lower 30

than both PVDF and PSF membranes. The pore size of CA demonstrates the CA is within the 31

microfiltration range with a mean flow pore size of 0.17 µm. The developed CA membrane shows 32

a promising oil/water emulsion permeability of 180 L m-2 h-1 bar-1 after five filtration cycles. 33

However, it still suffers a high degree of irreversible fouling (>90.0%), suggesting potential future 34

improvements in terms of membrane fouling management. Overall, this study demonstrates a 35

sustainable approach to addressing oil/water emulsion pollution treated CA membrane from 36

cigarette butt waste. 37

Keywords: cellulose acetate; cigarette waste; membrane fabrication; crossflow filtration; oily 38

wastewater; phase inversion 39

40

1. Introduction 41

Trillions of cigarette butts are hazardous material deposited annually in the 42

environment [1], and they have been identified as the most littered item worldwide [2]. 43

During the year 2016, 5.7 trillion cigarettes were consumed worldwide, and that about 44

97% of the cigarette filters were composed of cellulose acetate, a modified natural polymer 45

[3]. This figure is expected to increase by 1.6 times in 2025 [4]. The scientific community 46

Citation: Lastname, F.; Lastname, F.;

Lastname, F. Title. Polymers 2021, 13,

x. https://doi.org/10.3390/xxxxx

Academic Editor: Firstname

Lastname

Received: date

Accepted: date

Published: date

Publisher’s Note: MDPI stays

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Copyright: © 2021 by the authors.

Submitted for possible open access

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s/by/4.0/).

Polymers 2021, 13, x FOR PEER REVIEW 2 of 16

has been actively seeking economical and sustainable solutions to tackle the cigarette butt 47

waste pollution issue. To date, the alternatives to handle the pollution include 48

degradation, incineration, recycling, and landfilling. Several studies on converting the 49

waste cigarette butts into usable products were made in various fields, mainly in 50

environmental engineering, buildings and infrastructures, energy storage devices, 51

insecticide, and metallurgical industry [5,6]. Analysis of the potential recycling cigarette 52

butts waste in environmental engineering applications corresponds to about 14.0% of all 53

the possible applications [5]. The utilizations of cigarette butt waste have been mostly 54

focused in buildings and structure applications. 55

A large volume of oily wastewater is emitted into the environment. The oily 56

wastewater is mainly generated from industries such as petrochemical, petroleum 57

refineries, food manufacturing, and metallurgical [7]. Oily wastewater types include 58

unstable oil/water emulsion (or simply oil/water mixture), stable oil/water emulsion, and 59

free-floating oil [8]. The continuous and increasing discharge of oily wastewater can 60

severely endanger the ecosystem and pollute the environment. Without proper treatment, 61

emulsified oily wastewater can contaminate the groundwater resources in which drinking 62

water and agricultural production are affected [7]. 63

Conventional methods (flotation and coagulation) for the treatment of stable 64

oil/water emulsions are less effective in handling micron-sized emulsion droplets and 65

finely dispersed oil particles [9]. Membrane-based process is seen as one of the emerging 66

methods for treating oil/water emulsion wastewater that has shown effective in handling 67

low concentration of oil (<1000 ppm) in water [10–12]. It outstands the conventional 68

separation techniques for simplicity, continuous, faster, and cost-effectiveness due to their 69

low energy consumption. 70

The main component of cigarette butt is cellulose acetate (CA) [13], suitable to be 71

converted into polymeric membrane for liquid-based filtration [14]. Cellulose acetate is a 72

cellulose derivative, which possess good transparency and mechanical strength. Almost 73

90% of cigarettes are manufactured with cellulose acetate filter tips (cigarette butt) [15]. 74

Cigarette butts contain up to 96.0% of cellulose acetate that can be used to form membrane 75

material, as explored in this study. This wa, the circular economy concept can be 76

implemented by providing the opportunity to use cigarette butt waste into economically 77

attractive and usable products [16,17]. 78

A recent study showed that cellulose acetate from waste cigarette butt can be used as 79

raw material for the fabrication of nanofiber membrane [18]. The nanofiber achieved 80

99.9% of oil droplet separation efficiency when used to treat oil-in-water mixtures. The 81

oil/water mixture treated in this work was a less challenging feed of an oil/water mixture. 82

A more challenging feed in the form of oil/water emulsion separation has not been 83

addressed yet. Electrospun nanofiber membranes are notable for their superiority, high 84

efficiency, simplicity, and low cost [19]. In spite of that, one of the critical limitations of 85

the electrospun nanofiber membranes is their weak mechanical strength. They cannot be 86

used as a standalone system without an additional supporting layer and/or post- 87

treatment, normally in the form of non-woven [20,21]. Moreover, the electrospinning 88

process is relatively slow and requires a longer time to fabricate a membrane. Standard 89

fabrication time for a sheet of nanofiber net in a lab-scale set-up takes up to 100 hours. 90

Nonetheless, little attention has been given to other types of membrane fabrication 91

methods to develop CA-based membranes from waste cigarette butts. Therefore, this 92

study explored the application of cigarette butt as the polymer-based material for 93

membrane fabrication through the established phase inversion method [22] for treating 94

the challenging oil/water emulsion separation. Numerous researches have been 95

conducted to improvise the properties of the membrane from established polymer, such 96

as polyvinylidene difluoride (PVDF) and polysulfone (PSF) through modification of 97

fabrication parameters and post-treatments [23,24]. 98

In this study, we explore the utilization of waste cigarette butt as material for the 99

fabrication of phase inverted membranes. The resulting membrane was compared with 100

Polymers 2021, 13, x FOR PEER REVIEW 3 of 16

phase inverted membrane fabricated from commercial PSF and PVDF polymers, both 101

polymers are the most used in the commercial membranes for low-pressure filtration (i.e., 102

membrane bioreactor) [25]. After fabrication, all membranes were characterized in terms 103

of mean flow pore size, surface contact angle, morphology, and clean water permeability. 104

Finally, the filtration performance of the membranes was evaluated for filtration of 105

synthetic oil/water emulsion. This approach epitomized a circular economy in which 106

cigarette butt waste was converted into another valuable material for protecting nature 107

when applied for treating wastewater. 108

109

2. Materials and Methods 110

2.1 Materials 111

The dope solution compositions of the three membranes used in this study are 112

summarized in Table 1. The detail on fabrication and filtration of the plain PVDF and the 113

PSF membranes are available in our earlier reports [10,12]. For fabrication of CA-based 114

membrane, discarded cigarette butts were collected from public smoking areas. There was 115

no specific criterion for pre-screening of the cigarette butts collection. The collected 116

cigarette butts were first cleaned physically by removing any remaining tobacco, 117

wrapping papers, and burnt tips. The cigarette butts went through several cleaning cycles, 118

and each cycle consists of immersing and stirring the butts in boiling water. They were 119

dried thoroughly at 60°C in an air-circulating oven overnight to remove the moisture 120

content. The cleaned cigarette butts was dispersed in N,N-dimethylformamide (DMF, 121

Sigma-Aldrich, USA) solvent and cast atop a stainless steel mesh (37.0 µm mesh size, 122

Guangzhou, China) to provide mechanical strength. 123

Stabilized oil/water emulsion was synthesized according to earlier work [26] using 124

crude oil (obtained from a crude oil well in Malaysia), distilled water, and sodium dodecyl 125

sulfate (SDS, 98% purity, Sigma Aldrich). The SDS-to-oil ratio of 1:99 (w/w) was mixed in 126

water to obtain 1000 ppm stabilized emulsion via mechanical agitation at a stirring rate of 127

3500 rpm for 24 h. A small volume of feed samples was subsequently analyzed using 128

particle size and zeta potential analyzer (Malvern, Zetasizer Nano ZSP, Malvern, United 129

Kingdom) to map the oil droplet size distribution. The sizes of the droplets were in multi- 130

modals distribution with peaks at 0.25, 0.9, and 4.0 µm. 131

132

Table 1. Summary of materials and weight percentage in membranes evaluated in this study. 133

Membrane Polymer

Solvent Additives Support

CA 10 wt.% of

CA

90 wt.% of

DMF

- Stainless steel mesh

PSF 18 wt.% of

PSF

80.9 wt.% of

DMAc

1 wt.% of PEG

and

0.1 wt.% of LiCl

Nonwoven support

PVDF 15 wt.% of

PVDF

85 wt.% of

DMAc

-

Nonwoven support

CA: cellulose acetate, PSF: polysulfone, PVDF: polyvinylidene difluoride DMF: dimethylformamide, DMAc: dimethylacetamide, 134

PEG: polyethylene glycol. 135

2.2 Membrane preparation 136

For the preparation of CA-based membrane, the dope was prepared by dispersing 137

10 wt.% of the cleaned cigarette butt in a corresponding amount of DMF without any 138

additive (Table 1). The mixture was stirred for 24 h at 60° C to ensure the formation of a 139

homogeneous solution. The solution was degassed for several hours to release the 140

Polymers 2021, 13, x FOR PEER REVIEW 4 of 16

entrapped air bubbles before being used for membrane fabrication. The CA membrane 141

was synthesized via the phase inversion method with stainless steel mesh as the support. 142

The dope solution was poured on top of a flat stainless-steel mesh placed on the glass 143

plate. The dope solution was cast over the stainless steel mesh using a doctor blade with 144

a wet thickness of 330 µm to form a thin film. Subsequently, the casted film and the glass 145

plate were directly immersed in the non-solvent bath containing deionized water to 146

undergo the phase inversion. The resulting CA membrane was soaked in deionized water 147

until further use. 148

149

2.3 Membrane filtration set-up 150

The filtration system was operated under full recycling mode by constantly returning 151

the permeate to the feed solution after the volume was periodically (of every 10 mins) 152

measured. The set-up was used to analyze the membrane filtration performance in 153

treating synthetic oil/water emulsion. A peristaltic pump was used to provide a constant 154

transmembrane pressure of 0.2 bar while keeping the feed flowing through the system at 155

a linear velocity of 13.4 cm.s-1. The prepared membrane with an effective area of 36.5 cm2 156

was placed in between spacers in a lab-made filtration cell. The filtration was first 157

conducted using deionized water to determine the clean water permeability of the 158

membrane. Each filtration test was conducted for 60 minutes in which a queasy steady- 159

state permeability was obtained. 160

The filtration flux (𝐽𝑠, L m-2 h-1) and permeability (𝐿, L m-2 h-1 bar-1) were calculated 161

using Equation (1) and (2), respectively: 162

𝐽𝑠 =∆𝑉

𝐴𝑠 ∆𝑡 (1)

𝐿 =𝐽𝑠

∆𝑃 (2)

where ΔV is volume of the collected permeate (L), As is effective membrane area (m2), 163

ΔP is transmembrane pressure (0.2 bar), and Δt is filtration time (h). 164

2.4 Membrane characterization 165

The microstructures, cross-section, and surface morphology images of the resulting 166

membrane were processed using a scanning electron microscope (SEM, Zeiss Evo, 167

Germany). The samples were coated using gold to enhance the conductivity for obtaining 168

good images. The pore size distribution of the membranes was determined using a 169

capillary flow porometer (CFP, Porolux 1000, Berlin, Germany). The energy-dispersive X- 170

ray spectroscopy (EDS) was used to define the elemental composition near the surface of 171

the membrane samples. The hydrophilicity of the membrane surface was determined by 172

the static contact angle using a goniometer (Ramé-Hart 260, New Jersey, USA). The 173

chemical bonds of the CA membrane sample were identified using the Fourier transform 174

infrared spectrometer (FT-IR, Frontier 01 Perkin Elmer) in the spectra wavenumber range 175

of 400 to 4,000 cm-1. The concentration of oil content in the feed before and after the 176

filtration tests were studied using a UV-VIS spectrometer (Shimadzu UV-2600, Kyoto, 177

Japan) at a wavelength of 223 nm. 178

2.5 Membrane fouling identification 179

Before obtaining the clean water permeability, membrane compaction was 180

performed for 60 mins. The permeability was measured as the average value of the next 181

30 mins. After measuring the clean water permeability, the filtration of oil/water emulsion 182

feed was conducted for five cycles. Each cycle comprised of 30 mins filtration, followed 183

by 5 mins of membrane flushing with deionized water. From the five filtration cycles, 184

different types of fouling parameters were identified. The total fouling (𝑇𝐹, %), reversible 185

Polymers 2021, 13, x FOR PEER REVIEW 5 of 16

(𝑅𝐹, %) and irreversible fouling (𝐼𝑅,%) of the membrane were determined using Equations 186

(3), (4) and (5), respectively: 187

𝑇𝐹𝑛 =𝐿𝑜−𝐿𝑛

𝐿𝑜 (3)

𝑅𝐹𝑛 =𝐿𝑜(𝑛)−𝐿𝑜(𝑛−1)

𝐿𝑛 (4)

𝐼𝑅𝑛 =𝐿𝑛 − 𝐿𝑜(𝑛)

𝐿𝑛

(5)

188

where n is number of filtration cycle, 𝐿𝑜 is the clean water permeability at the beginning 189

of the filtration, 𝐿𝑛 is average permeability at cycle n, 𝐿𝑜(𝑛) is the permeability of clean 190

water at cycle n, 𝐿𝑜(𝑛−1) is the permeability of oil-in-water emulsion filtration at cycle n-1. 191

192

3. Results and Discussion 193

3.1 Surface and cross-section morphologies 194

195

196 Figure 1. Surface and cross-section SEM images of the membrane samples. 197

Figure 1 shows the morphological structure of the developed CA, PSF, and PVDF 198

membranes. Based on the top surface SEM images, all samples pose visible surface pores 199

homogeneously distributed. They show the typical morphology of membranes prepared 200

by non-solvent induced phase separation. Most importantly, despite being prepared from 201

waste cigarette butt, the CA membrane also poses good surface property like the ones 202

prepared from the commercial PVDF and PSF polymer, typically used for membranes 203

fabrication. The finding on the microstructure suggesting the potential of a waste cigarette 204

butt for membrane fabrication, which can be applied for oil/water emulsion filtration. The 205

surface pores are within a size range far below most of the oil droplets presented in the 206

oil/water emulsion feed used in this study. 207

The cross-section images of all membranes show equally asymmetrical morphology, 208

a typical structure of membranes prepared from non-solvent induced phase separation 209

under instantaneous demixing [27], in which a dense surface morphology is supported by 210

a more porous structure underneath. The large surface pores of the CA membrane are all 211

Polymers 2021, 13, x FOR PEER REVIEW 6 of 16

within the microfiltration range, which also suggests the instantaneous demixing phase 212

separation mechanism. A recent report on the fabrication of CA membrane from 213

commercial CA polymer showed symmetric morphology since it was prepared from 214

different solvent/nonsolvent systems and different polymer concentrations [14]. Detailed 215

discussion on relationships between polymer/solvent/nonsolvent system can be found 216

elsewhere [14,24,28]. The finding suggests that irrespective of the source (i.e., waste 217

cigarette butt), CA membrane could be prepared using the phase inversion method 218

resulting reliable membrane effectively used for filtration, as demonstrated in Section 3.7. 219

3.2 Membrane pore size and distribution 220

221

222

Figure 2. The pore size distribution of the developed cellulose acetate (CA), polysulfone (PSF), and 223

polyvinylidene difluoride (PVDF) membranes. 224

225

Figure 2 shows the pore size distribution of the three membrane samples evaluated 226

using a CFP. The y-axis of the figure show the actual distribution of pore of certain size, 227

not the frequency distribution found in a typical histogram. The pore distribution of all 228

memnbrane samples skew to the left indicating of higher populations of smaller pores. 229

The cigarette butt–based CA membrane poses a high pore size population at around 0.10- 230

0.15 µm. The pore size range of the cigarette butt–based CA membrane is suitable for 231

handling the oil/water emulsion because the pores theoretically could retain emulsion 232

droplets with sizes larger than the membrane pore sizes. The sizes of the oil droplets in 233

emulsion are normally in the range of 0.1 to 10 µm [29]. Most of the oil droplets can be 234

effectively removed with a membrane of pore size in the range of 2 to 100 nm. The 235

membrane works based on the size exclusion theory, in which the membrane material 236

rejects particles larger than the pore size. Higher mean flow pore sizes are shown by the 237

PSF and PVDF membranes at 0.127 and 0.210 µm, respectively. It was reported that the 238

typical commercial microfiltration CA-based membrane has a pore size of 0.470 µm [30], 239

most likely because of some differences in fabrication parameters. Indeed, further 240

exploration can still be done to fine-tune the properties of a cigarette butt CA-based 241

membranes according to the required specifications as suggested elsewhere [31–33]. 242

0

10

20

30

40

50

60

0 0.2 0.4

Dis

trib

uti

on

(%)

Pore Size Diameter (µm)

PSF

PVDF

CA

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243

Figure 3. The mean pore size distribution of the cellulose acetate (CA), polysulfone (PSF), and 244

polyvinylidene difluoride (PVDF) membranes. 245

Figure 3 depicts the mean pore size distribution of CA, PSF, and plain PVDF analyzed 246

with CFP. The CFP test accurately captures the pore size across the thickness and the size 247

distribution shown in Figure 2. It shows that the plain PVDF membrane exhibits the 248

largest mean flow pore size of 0.2206 µm in comparison to CA and PSF, with mean flow 249

pore size of 0.17 and 0.1556 µm, respectively. The SEM images of the plain PVDF 250

membrane show poor surface pore visibility. Figure 3 shows that the pore size of the 251

membranes is comparable and all are expected to effectively retain oil droplets in the 252

oil/water emulsion feeds. In addition to the mean flow pore size and pore size distribution, 253

the specific number of pore per unit of membrane surface is also important to govern the 254

permeability and can distinguish the throughput of membranes despite having similar 255

pore size and distributions. 256

3.3 Surface contact angle 257

258

Figure 4. Static contact angle of the developed cellulose acetate (CA), polysulfone (PSF) and 259

polyvinylidene difluoride (PVDF) membranes. 260

261

Figure 4 shows the static water contact angle for the three membrane samples used 262

in this study. The static water contact angle is essential in determining the permeability 263

and fouling properties of a membrane. A membrane is considered hydrophilic when the 264

contact angle falls between 0° to 90°. Membranes with hydrophilic properties are ideal in 265

oil/water emulsion treatment when water is the component that is permeating through 266

the membrane pore and vice versa [34,35]. Hydrophilic surface attracts water by creating 267

a hydration layer and prevents oil droplet interaction with the membrane surface, hence 268

improvingimproving oil droplet rejection [36]. As shown in Figure 4, PVDF membrane 269

0

0.1

0.2

0.3

CA PSF PVDF

Mea

n fl

ow

po

re s

ize

(µm

)

Membrane samples

0

20

40

60

80

100

CA PSF PVDF

Surf

ace

Co

nta

ct A

ngl

e ( )

Membrane samples

Polymers 2021, 13, x FOR PEER REVIEW 8 of 16

demonstrates the most hydrophobic characteristic with a water contact angle of 81.59°, 270

attributed to the low polymer surface free energy [37]. This is followed by CA and PSF 271

membranes with the surface water contact angles of 74.5° and 70.23°, respectively. The 272

surface water contact angle of plain CA membrane from commercial polymers in this 273

study is within the range reported earlier of 50-60° [38–40], which can be attributed to 274

variation surface structure and fabrication parameters and possibly due to presence of 275

impurities that can be further investigated as the follow up study. These findings are 276

encouraging and show a CA membrane based from cigarette butt waste potentially 277

possess a high clean water permeability and good anti fouling property, at least when 278

compared with the PVDF and PSF membranes samples used as reference in this study. 279

3.4 Fourier transform infrared 280

The FT-IR spectra in Figure 5 depicts the chemical composition of the prepared 281

cigarette butt-based CA membrane. The FT-IR spectrum of CA shows a peak absorption 282

band at 1747, 1230, and 1050 cm-1 which is assigned to the C=O carbonyl stretching, C-O 283

stretching, and CO-O-CO stretching. The peaks at 1371 and 2920 cm−1 are attributed to the 284

C-O group and aliphatic group (C-H), respectively. And broad peak at around 3500 cm-1 285

represents the O-H group. Similar findings were reported by Liu et al. that attributed the 286

presence of carbonyl stretching, symmetric, and asymmetric stretching vibrations of C-O- 287

C, respectively, in nanofiber membrane from waste cigarette butt [18]. 288

289

Figure 5. FT-IR spectra of the cellulose acetate membrane. 290

291

The spectra shown in Figure 5 resemble the one obtained for phase inverted 292

membrane prepared from commercial CA polymer [40,41]. The presence of impurities is 293

hardly seen from the spectra, indicating that the spectra associate with them might be 294

overlapping with spectra associated with CA. Visually, the presence of impurities could 295

be seen from the grey color of the cigarette butt CA-based membrane. The presence of 296

impurities might affect the resulting membrane properties (i.e., higher water contact 297

angle) and the purification process is thus recommended as the follow-up studies. 298

Polymer purification was shown effective in improving the structure and performance of 299

the resulting membranes [42]. 300

3.5 Energy Dispersive X-Ray Spectroscopy 301

Table 2 shows the distribution of elemental composition for CA, PSF, and PVDF 302

membranes obtained from EDS mapping. It is observed that the oxygen originating from 303

the hydroxyl group in CA has the highest composition at 48.2%. It is slightly higher than 304

the one obtained from X-ray photoelectron spectroscopy of 42.0% obtained elsewhere [40]. 305

This result indicated the presence of hydrophilic functional groups in the CA membrane, 306

which justifies the CA membrane has higher hydrophilicity properties than the PSF and 307

Polymers 2021, 13, x FOR PEER REVIEW 9 of 16

the PVDF membranes. The presence of carbon and oxygen is supported by FT-IR analysis. 308

In contrast, the static contact angle measurement suggests that the PVDF membrane 309

demonstrates the most hydrophilic characteristic with a contact angle of water of 81.59°. 310

The abundance of oxygen element in the CA membrane can further be explored to 311

enhance the surface hydrophilicity. 312

313

Table 2. The elemental composition of the cellulose acetate (CA), polysulfone (PSF), and 314

polyvinylidene difluoride (PVDF) membranes. 315

Membrane Composition (%)

C F O S

CA 51.60 0.00 48.20 0.00

PSF 69.02 0.00 26.05 4.92

PVDF 55.55 42.84 1.61 0.00

316

3.6 Clean water permeability 317

318

319

Figure 6. Clean water permeability of the cellulose acetate (CA), polysulfone (PSF), and 320

polyvinylidene difluoride (PVDF) membranes. 321

322

Figure 6 shows that the CA membrane outperforms the rest in filtration performance 323

by having the highest permeability compared to PSF and PVDF membranes. Clean water 324

permeability involves the passage of water molecules through the membrane under 325

crossflow filtration. The CA membrane showed the water permeability of 1658 L m-2 h-1 326

bar-1 significantly higher than the PSF and PVDF membranes clean water permeability of 327

446 L m-2 h-1 bar-1 and 175 L m-2 h-1 bar-1, respectively. 328

When considering the pore size and distribution of the three membrane samples 329

evaluated in this study, significantly high permeability shown by CA membrane can be 330

ascribed by their low surface water contact angle (Figure 4) combined with higher surface 331

pore population. Some membranes can show similar pore size and distribution but differ 332

in pore number, as detailed in an earlier report [43]. When evaluating the surface SEM 333

image in Figure 1, it can be seen that the CA membrane's surface pores are highly 334

populated compared to the rests. 335

3.7 Filtration performance 336

0

400

800

1200

1600

2000

CA PSF PVDF

Pe

rme

ab

ilit

y (

Lm-2

h-1

ba

r -1

)

Membrane samples

Polymers 2021, 13, x FOR PEER REVIEW 10 of 16

337 Figure 7. The permeability of the cellulose acetate (CA), polysulfone (PSF), and polyvinylidene 338

difluoride (PVDF) membranes for five cycles in thirty minutes oil-in-water emulsion and five 339

minutes in clean water as a function of filtration time. 340

341

Figure 7 shows that the CA poses the highest oil/water emulsion permeability for the 342

first 50 min of filtration, maintained at a value of 180 L m-2 h-1 bar-1 at the end of the 343

subsequent filtration cycles. The high performance of the CA membrane can be attributed 344

to the high oxygen content in the membrane that imposes surface hydrophilicity which is 345

beneficial for repelling deposited oil droplets when treating the oil/water emulsion and 346

forming a hydration layer on the membrane surface [36]. The membrane surface has high 347

surface porosity (from a high number of the surface pore, see ), as shown on the SEM 348

images in Figure 1, which could offer a better oil/water emulsion permeability than the 349

PSF and the PVDF membranes. The clean water flushing introduced at each filtration cycle 350

helps to improve the permeability of the membrane and remove the oily foulant and 351

reduce the fouling effect on the membrane. It can be observed the water flushing at cycle 352

2, 3, 4, and 5 improve the subsequent permeability of the membrane in oil/water emulsion. 353

However, the water flushing in cycle 1 does not exhibit an increase of permeability. This 354

may occur due to the strong oil adhesion on the membrane surface that has caused the 355

emulsion permeability to dramatically decrease. 356

In another study, the permeability of the oil/water emulsion for commercial CA 357

membrane in the first cycle is 1900 Lm-2 h-1 bar-1. After the first flushing, the permeability 358

decreased significantly to 370 Lm-2 h-1 bar-1, following the third cycle of 90 Lm-2 h-1 bar-1. 359

The subsequent cycles show no permeability, which demonstrated the oil particles have 360

wholly clogged the membrane pores suggesting severe membrane fouling also happen to 361

a plain CA membrane made from commercial polymer [30]. Although the commercial CA 362

membrane has a high permeability at the initial phase, it is worth noting that the 363

permeability had a steep decrease. When compared to the CA membrane from cigarette 364

waste, the developed membrane exhibited a relatively slow decrease in the whole five 365

cycles. This constitutes an interesting phenomenon as the developed CA is made of 366

cigarette butt waste. Further comparison with PSF and PVDF membranes optimized for 367

oil/water emulsion filtration was reported earlier [10,42]. The permeability is comparable 368

with the plain CA membranes developed from cigarette butt waste reported in the present 369

study. It suggests that the CA-based membrane from cigarette butt, can further be 370

developed to enhance its filtration performance via fabrication parameter optimization or 371

surface modifications. 372

373

374

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3.8 Rejection performance 375

376

377 Figure 8. The oil rejection of PW filtration using the cellulose acetate (CA), polysulfone (PSF), and 378

polyvinylidene difluoride (PVDF) membranes. 379

380 To evaluate the oil separation efficiency, the oil rejection performances of the CA 381

membrane was evaluated and compared with PSF and PVDF membranes. The CA 382

membrane exhibits an excellent total oil rejection of 91.5%. This shows that the CA 383

membrane developed from cigarette waste is comparable to the established PSF 384

membrane that has achieved the rejection efficiency of 94.0%. In addition, CA could be a 385

promising candidate in achieving a large-scale separation of oil/water emulsion for its 386

greater oil rejection than the PVDF membrane. A study by Liu et al. found that the 387

stainless steel mesh (size 300 and 2300) alone could not separate the oil/water mixture well 388

as the oil and water passed through the mesh unobstructively [18]. 389

A similar study by Ifelebuegu et.al using waste cigarette butt in oil spill clean-up 390

found that waste filters adsorbed 16 to 26 times their weights in various oils, which is a 391

better oil sorption performance than those commercial adsorbents. It also reported that 392

the sorption capacity did not significantly deteriorate after 20 cycles of reuse, with up to 393

75% sorption capacity retained [44]. Nair reported the highest absorption of dye using the 394

CA membrane prepared from cigarette buds was obtained in slightly acidic conditions 395

with the pH of 6.15 [45]. 396

The finding suggests the effectiveness of the developed CA membrane to separate oil 397

droplets. The good separation can be ascribed from the relatively large difference between 398

the mean flow pore size of 0.17 µm and most of the oil droplets >0.25 µm. Those 399

differences allow the separation through size exclusion mechanisms in which oil droplets 400

were retained on the top of the membrane surface [35,46]. 401

402

403

Polymers 2021, 13, x FOR PEER REVIEW 12 of 16

3.9 Membrane fouling analysis 404

405

Figure 9. The evolution of membrane fouling in terms of reversible and irreversible fouling. 406

407

Figure 9 shows the analysis of membrane fouling based on its reversibility for CA 408

compared to the PSF and the PVDF membranes. As expected, the total fouling for all three 409

types of membranes showed an increasing trend with the increasing filtration cycles. The 410

trend of multiple cycle performance is consistent with our earlier report treating the same 411

feed following similar filtration cycles [10,12,47,48]. The three membranes pose quite 412

distinct fouling reversibility. The total fouling depicted by PVDF at each cycle is relatively 413

lower than the PSF and the CA membranes, indicating a lower degree of permeability loss 414

and better antifouling properties. However, when judging from the actual permeability 415

data in Figure 7, the performance of the PVDF membrane is comparable with the CA 416

membrane. The low degree of fouling in PVDF membrane compared to others is due to 417

its relatively low clean water permeability compared to others (Figure 6). Therefore, the 418

fouling parameters become low since the oil/water emulsion permeability was compared 419

to the initial clean water permeability (Equations 3-5). On the contrary, both CA and PSF 420

demonstrated high total fouling since they pose high clean water permeability 421

accompanied by similar oil/water emulsion permeability. 422

It is observed from Figure 9 that the membrane fouling in CA and PSF are dominated 423

by irreversible fouling. The CA suffers a relatively high degree of irreversible fouling since 424

the first filtration cycle. It should also be noted that CA has five-folds higher clean water 425

permeability than PSF and PVDF at the initial cycle. It is speculated that the high fouling 426

rate of CA was caused by the rapid compaction of permanent foulant trapped in the pores 427

that occurred during the first cycle resulting in a lower oil/water emulsion permeability. 428

After the first cycle, the rate of foulant accumulation is very small, indicating that the 429

foulant was well consolidated. It is wort noting that the occurrence of membrane fouling 430

can be well managed by implementing membrane cleaning cycles. Under proper fouling 431

management, the lifespan of a membrane can be over 15 years [49]. 432

Polymers 2021, 13, x FOR PEER REVIEW 13 of 16

The finding on high degree of irreversible membrane fouling during the early stage 433

of filtration indicates the possibility of further developing phase inverted cigarette butt- 434

based CA membrane, focusing on combating the irreversible fouling. As demonstrated in 435

earlier report, the incorporation of zirconia (ZrO2) particles in CA casting solution resulted 436

in a decrease in fouling resistance. The total fouling resistance for pure CA membrane is 437

7.19 × 1010 m-1. The addition of 7 wt.% of ZrO2 decreased the total fouling resistance to 2.58 438

× 1010 m-1 [50]. This may due to the increase in hydrophilicity of CA membrane, which 439

increases the interaction of the molecules on the membrane surface. 440

4. Conclusions 441

This study unravels the potential of CA from cigarette butt waste as material for 442

membrane fabrication for oil/water emulsion treatment. This utilization of waste can 443

alleviate the environmental problems from cigarette butt waste as well tackling the issue 444

of oil/water emulsion. The CA-based membrane was successfully fabricated via the phase 445

inversion method with a typical structure formed from the instantaneous demixing 446

process. The findings show that CA membrane poses hydrophilicity properties with a 447

contact angle of 74.5°, lower than both PVDF and PSF membranes used as reference. The 448

pore size and distribution are suitable for oil/water separation. Despite being prepared 449

from a waste cigarette, CA also poses good surface property similar to the ones prepared 450

from commercial PVDF and PSF polymer with equally asymmetric morphology. The pore 451

size of CA demonstrates the CA is within the microfiltration range. The developed CA 452

membrane shows a promising flux of 180 Lm-2 h-1 after multiple filtration cycles of 453

oil/water emulsion. However, it still suffers a high degree of irreversible fouling (>90.0 %), 454

suggesting potential for future improvement through optimization of fabrication 455

parameters or via surface modification. Overall results demonstrate a sustainable 456

approach in handling oil/water emulsion pollution issue by treatment using CA 457

membrane derived from cigarette butt waste. 458

Author Contributions: Data curation, methodology, validation, writing—original draft 459 preparation, A.D. and C.L.L., Supervision, conceptualization, methodology, validation, writing— 460 review and editing, M.R.B.; validation, writing—review and editing, S.P., K.A.K. and S.S.; 461 methodology and writing—review and editing, T.N. and K.F. All authors have read and agreed to 462 the published version of the manuscript. 463

Funding: This research received no external funding. 464

Institutional Review Board Statement: 465

Informed Consent Statement: 466

Data Availability Statement: 467

Acknowledgments: 468

Conflicts of Interest: The authors declare no conflict of interest. 469

470

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S.-H.; Lee, K.-R. Modifying Cellulose Acetate Mixed-Matrix Membranes for Improved Oil–Water Separation: 568

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Oleophilic Sorbent from Waste Cigarette Filters for the Sequestration of Oil Pollutants from an Aqueous 582

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Mohshim, D.F. Polyvinylidene Fluoride Membrane Via Vapour Induced Phase Separation for Oil/Water Emulsion 590

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Development of Hydrophilic PVDF Membrane Using Vapour Induced Phase Separation Method for Produced 593

Water Treatment. Membranes 2020, 10, 121, doi:10.3390/membranes10060121. 594

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50. Arthanareeswaran, G.; Thanikaivelan, P. Fabrication of Cellulose Acetate–Zirconia Hybrid Membranes for 597

Ultrafiltration Applications: Performance, Structure and Fouling Analysis. Sep. Purif. Technol. 2010, 74, 230–235, 598

doi:10.1016/j.seppur.2010.06.010. 599

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polymers-1223672

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DOI 10.3390/polym13121907

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Abstract (https://www.mdpi.com/2073-4360/13/12/1907) HTMLversion (https://www.mdpi.com/2073-4360/13/12/1907/htm)PDF version (https://www.mdpi.com/2073-4360/13/12/1907/pdf) Manuscript (https://www.mdpi.com/2073-4360/13/12/1907/manuscript)

Article type Article

Title Cigarette Butt Waste as Material for Phase Inverted MembraneFabrication Used for Oil/Water Emulsion Separation

Journal Polymers (https://www.mdpi.com/journal/polymers)

Volume 13

Issue 12

Section Polymer Applications(https://www.mdpi.com/journal/polymers/sections/Polymer_Applications)

Special Issue Polymer Nanocomposite Membranes for EnvironmentalApplications(https://www.mdpi.com/journal/polymers/special_issues/Polymer_Nanocomposite_Membranes_Environmental_Applications)

Abstract The increasing rate of oil and gas production has contributed toa release of oil/water emulsion or mixtures to the environment,becoming a pressing issue. At the same time, pollution of thetoxic cigarette butt has also become a growing concern. Thisstudy explored utilization of cigarette butt waste as a source ofcellulose acetate-based (CA) polymer to develop a phaseinverted membrane for treatment of oil/water emulsion andcompare it with commercial polyvinylidene difluoride (PVDF) andpolysulfone (PSF). Results show that the CA-based membranefrom waste cigarette butt offers an eco-friendly material withoutcompromising the separation efficiency, with a pore size rangesuitable for oil/water emulsion filtration with the rejection of>94.0%. The CA membrane poses good structural propertysimilar to the established PVDF and PSF membranes withequally asymmetric morphology. It also poses hydrophilicityproperties with a contact angle of 74.5°, lower than both PVDFand PSF membranes. The pore size of CA demonstrates thatthe CA is within the microfiltration range with a mean flow poresize of 0.17 µm. The developed CA membrane shows apromising oil/water emulsion permeability of 180 L m h barafter five filtration cycles. However, it still suffers a high degree ofirreversible fouling (>90.0%), suggesting potential future

−2 −1 −1

improvements in terms of membrane fouling management.Overall, this study demonstrates a sustainable approach toaddressing oil/water emulsion pollution treated CA membranefrom cigarette butt waste.

Keywords cellulose acetate; cigarette waste; membrane fabrication;crossflow filtration; oily wastewater; phase inversion

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Author Information

SubmittingAuthor

Muhammad Roil Bilad

CorrespondingAuthors

Aris Doyan, Muhammad Roil Bilad

Author #1 Aris Doyan

Affiliation 1. Master of Science Education Program, University of Mataram,Jl. Majapahit No. 62, Mataram 83125, Indonesia2. Physics Education, FKIP, University of Mataram, Jl. MajapahitNo. 62, Mataram 83125, Indonesia

E-Mail aris_doyan@unram.ac.id

Author #2 Chew Lee Leong

Affiliation 3. Department of Chemical Engineering, Universiti TeknologiPETRONAS, Bandar Seri Iskandar 32610, Malaysia

E-Mail leongchewlee@gmail.com

Author #3 Muhammad Roil Bilad

Affiliation 3. Department of Chemical Engineering, Universiti TeknologiPETRONAS, Bandar Seri Iskandar 32610, Malaysia4. Faculty of Applied Science and Technology, UniversitasPendidikan Mandalika (UNDIKMA) Jl Pemuda No 59A

Pendidikan Mandalika (UNDIKMA), Jl. Pemuda No. 59A,Mataram 83126, Indonesia5. Faculty of Integrated Technologies, Universiti BruneiDarussalam, Jalan Tungku Link, Gadong BE1410, Brunei

E-Mail muhammadoilbilad@ikipmataram.ac.id

Author #4 Kiki Adi Kurnia

Affiliation 6. Department of Chemistry, Faculty of Mathematics and NaturalSciences, Institut Teknologi Bandung, Bandung 40132,Indonesia

E-Mail kurnia.kikiadi@gmail.com

Author #5 Susilawati Susilawati

Affiliation 1. Master of Science Education Program, University of Mataram,Jl. Majapahit No. 62, Mataram 83125, Indonesia2. Physics Education, FKIP, University of Mataram, Jl. MajapahitNo. 62, Mataram 83125, Indonesia

E-Mail susilawatihambali@unram.ac.id

Author #6 Saiful Prayogi

Affiliation 4. Faculty of Applied Science and Technology, UniversitasPendidikan Mandalika (UNDIKMA), Jl. Pemuda No. 59A,Mataram 83126, Indonesia

E-Mail saifulprayogi@ikipmataram.ac.id

Author #7 Thanitporn Narkkun

Affiliation 7. National Nanotechnology Center (NANOTEC), NationalScience and Technology Development Agency (NSTDA), 111Thailand Science Park, Pathum Thani 12120, Thailand

E-Mail thanitporn.nar@ncr.nstda.or.th

Author #8 Kajornsak Faungnawakij

Affiliation 7. National Nanotechnology Center (NANOTEC), NationalScience and Technology Development Agency (NSTDA), 111Thailand Science Park, Pathum Thani 12120, Thailand

E-Mail kajornsak@nanotec.or.th

Manuscript Information

ReceivedDate

30 April 2021

Revised Date 2 June 2021

AcceptedDate

3 June 2021

PublishedDate

8 June 2021

Submissionto First

Decision(Days)

10

Submissionto Publication

(Days)

38

(https://orcid.org/0000-0002-6858-0510)

(https://orcid.org/0000-0001-8858-5282)

(https://orcid.org/0000-0002-4724-0613)

Round ofRevision

2

Size of PDF 4040 KiB

Word Count 5205

Page Count 15

Figure Count 10

Table Count 2

ReferenceCount

51

Editor Decision

Decision Accept after minor revision

Comments The authors have tried to address the concerns raised. Followingvery minor corrections are needed: -There should be aschematic for the membrane fabrication -The quality (in text) inthe figure should be improved -Some of the relevant referencesmay be cited such as Polymers 2021, 13(11), 1743; Polymers2021, 13(11), 1716; Materials Today Chemistry 17, 100302(2020); Chemical Reviews 120 (17), 9304–9362 (2020)

DecisionDate

27 May 2021

Review Report

Reviewer 1 Review Report (Round 1) (/user/manuscripts/review/17841888?report=11925566)

Review Report (Round 2) (/user/manuscripts/review/17841888?report=12202637)

Reviewer 2 Review Report (Round 1) (/user/manuscripts/review/17842024?report=11925660)

Review Report (Round 2) (/user/manuscripts/review/17842024?report=12202628)

APC information

Journal APC: 2,200.00 CHF

DiscountVoucher:

707b171a05fefd01 (500.00 CHF) (mroil.bilad@utp.edu.my)

TotalPaymentAmount:

1,700.00 CHF

Previously Published Papers

Susilawati, S.; Prayogi, S.; Arif, M.F.; Ismail, N.M.; Bilad, M.R.; Asy’ari, M. Optical Properties andConductivity of PVA–H PO (Polyvinyl Alcohol–Phosphoric Acid) Film Blend Irradiated by γ-Rays.Polymers 2021, 13, 1065. doi: 10.3390/polym13071065 (https://doi.org/10.3390/polym13071065)

Mohammed, H.G.; Albarody, T.M.B.; Susilawati, S.; Gohari, S.; Doyan, A.; Prayogi, S.; Bilad, M.R.;Alebrahim, R.; Saeed, A.A.H. Process Optimization of In Situ Magnetic-Anisotropy Spark PlasmaSintering of M-Type-Based Barium Hexaferrite BaFe O . Materials 2021, 14, 2650. doi:10.3390/ma14102650 (https://doi.org/10.3390/ma14102650)

3 4

12 19

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Doyan, A.; Susilawati, S.; Prayogi, S.; Bilad, M.R.; Arif, M.F.; Ismail, N.M. Polymer Film Blend ofPolyvinyl Alcohol, Trichloroethylene and Cresol Red for Gamma Radiation Dosimetry. Polymers2021, 13, 1866. doi: 10.3390/polym13111866 (https://doi.org/10.3390/polym13111866)

Related Papers Published in MDPI Journals

If you have any questions or concerns, please do not hesitate to contact polymers@mdpi.com (mailto:polymers@mdpi.com).

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Journal Polymers (https://www.mdpi.com/journal/polymers) (ISSN 2073-4360)

ManuscriptID

polymers-1223672

Type Article

Number ofPages

16

Title Cigarette Butt Waste as Material for Phase Inverted MembraneFabrication Used for Oil/Water Emulsion Separation

Authors Aris Doyan * , Chew Lee Leong , Muhammad Roil Bilad * , KikiAdi Kurnia , Susilawati Susilawati , Saiful Prayogi , ThanitpornNarkkun , Kajornsak Faungnawakij

Abstract The increasing rate of oil and gas production has contributed in arelease of oil-in-water emulsion or mixtures to the environmentwhich has become a pressing issue. At the same time, pollutionof the toxic cigarette butt has also become the growing concern.This study explores utilization of cigarette butt waste as sourceof cellulose acetate-based (CA) polymer to develop phaseinverted membrane for treatment of oil/water emulsion andcompared with commercial polyvinylidene difluoride (PVDF) andpolysulfone (PSF). Results show that CA-based membrane fromwaste cigarette butt offers an eco-friendly material withoutcompromising the separation efficiency, with pore size rangesuitable for oil/water emulsion filtration with rejection of >94.0%.The CA membrane poses good structural property like that ofestablished PVDF and PSF membranes with equally asymmetricmorphology. It also poses hydrophilicity properties with contactangle of 74.5°, lower than both PVDF and PSF membranes. Thepore size of CA demonstrates the CA is within the microfiltrationrange with mean flow pore size of 0.17 µm. The developed CAmembrane shows a promising oil/water emulsion permeability of180 L m-2 h-1 bar-1 after five filtration cycles. However, it stillsuffers a high degree of irreversible fouling (>90.0%), suggestingpotential for future improvements. Overall, this studydemonstrates a sustainable approach in addressing issue ofoil/water emulsion pollution treated CA membrane from cigarettebutt waste.

The coverletter for this review report has been saved in thedatabase. You can safely close this window.

Authors' Responses to Reviewer's Comments (Reviewer 1)

Author'sNotes

Please see the attachment.

Author'sNotes File

Report Notes (/user/review/displayFile/17841888/khBHsV4W?file=author-coverletter&report=11925566)

Review Report Form

Englishlanguageand style

( ) Extensive editing of English language and style required ( ) Moderate English changes required (x) English language and style are fine/minor spell checkrequired ( ) I don't feel qualified to judge about the English languageand style

Yes Can beimproved

Must beimproved

Notapplicable

Does the introduction provide sufficient

background and include all relevant references?(x) ( ) ( ) ( )

Is the research design appropriate? (x) ( ) ( ) ( )

Are the methods adequately described? ( ) (x) ( ) ( )

Are the results clearly presented? ( ) (x) ( ) ( )

Are the conclusions supported by the results? ( ) (x) ( ) ( )

Commentsand

Suggestionsfor Authors

The manuscript entitled: "Cigarette Butt Waste as Material forPhase Inverted Membrane Fabrication Used for Oil/WaterEmulsion Separation" is an extended work dealing with thesustainable use of cigarette butt that are normal wastes for thefabrication of membranes for oil/water separation.

The manuscript deserves to be suggested for publication aftersome minor clarifications to the following points:

1. The pore size distribution image is very strange. Can theauthors state if there is a specific function followed for thepore sizes?

2. What is the process of obtaining the cigarette butts?3. Did the authors consider comparing pure CA and also CA for

cigarette butts?4. It is not clear how the cigarette-butt CA polymer was

recovered. Please give some details of the cleaning process.5. Fouling experiments indicate that the membranes will end up

in the waste after the operation which is somehowcontradictory to the concept of this work. Is there anymodification method of the produce CA membranes for thebetter rinsing of the membranes after the use for theseparation of oil/water?

6. last but not least, sustainability is a key factor, however,energy efficiency is also extremely important. The processproposed for the cleaning of the cigarette butts seems to beof high costs due to the use of cleaners and also of thematerial for a short time due to the feature of the separation.What do the authors believe, is this method good in order toobtain a sustainable concept or an optimized one?

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SubmissionDate

30 April 2021

Date of thisreview

11 May 2021 01:41:47

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Journal Polymers (https://www.mdpi.com/journal/polymers) (ISSN 2073-4360)

ManuscriptID

polymers-1223672

Type Article

Number ofPages

16

Title Cigarette Butt Waste as Material for Phase Inverted MembraneFabrication Used for Oil/Water Emulsion Separation

Authors Aris Doyan * , Chew Lee Leong , Muhammad Roil Bilad * , KikiAdi Kurnia , Susilawati Susilawati , Saiful Prayogi , ThanitpornNarkkun , Kajornsak Faungnawakij

Abstract The increasing rate of oil and gas production has contributed in arelease of oil-in-water emulsion or mixtures to the environmentwhich has become a pressing issue. At the same time, pollutionof the toxic cigarette butt has also become the growing concern.This study explores utilization of cigarette butt waste as sourceof cellulose acetate-based (CA) polymer to develop phaseinverted membrane for treatment of oil/water emulsion andcompared with commercial polyvinylidene difluoride (PVDF) andpolysulfone (PSF). Results show that CA-based membrane fromwaste cigarette butt offers an eco-friendly material withoutcompromising the separation efficiency, with pore size rangesuitable for oil/water emulsion filtration with rejection of >94.0%.The CA membrane poses good structural property like that ofestablished PVDF and PSF membranes with equally asymmetricmorphology. It also poses hydrophilicity properties with contactangle of 74.5°, lower than both PVDF and PSF membranes. Thepore size of CA demonstrates the CA is within the microfiltrationrange with mean flow pore size of 0.17 µm. The developed CAmembrane shows a promising oil/water emulsion permeability of180 L m-2 h-1 bar-1 after five filtration cycles. However, it stillsuffers a high degree of irreversible fouling (>90.0%), suggestingpotential for future improvements. Overall, this studydemonstrates a sustainable approach in addressing issue ofoil/water emulsion pollution treated CA membrane from cigarettebutt waste.

Review Report Form

Englishlanguageand style

( ) Extensive editing of English language and style required ( ) Moderate English changes required (x) English language and style are fine/minor spell checkrequired ( ) I don't feel qualified to judge about the English languageand style

Yes Can beimproved

Must beimproved

Notapplicable

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Does the introduction provide sufficient

background and include all relevant references?(x) ( ) ( ) ( )

Is the research design appropriate? (x) ( ) ( ) ( )

Are the methods adequately described? (x) ( ) ( ) ( )

Are the results clearly presented? (x) ( ) ( ) ( )

Are the conclusions supported by the results? (x) ( ) ( ) ( )

Commentsand

Suggestionsfor Authors

The revised version can now get accepted

SubmissionDate

30 April 2021

Date of thisreview

19 May 2021 20:17:08

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Journal Polymers (https://www.mdpi.com/journal/polymers) (ISSN 2073-4360)

ManuscriptID

polymers-1223672

Type Article

Number ofPages

16

Title Cigarette Butt Waste as Material for Phase Inverted MembraneFabrication Used for Oil/Water Emulsion Separation

Authors Aris Doyan * , Chew Lee Leong , Muhammad Roil Bilad * , KikiAdi Kurnia , Susilawati Susilawati , Saiful Prayogi , ThanitpornNarkkun , Kajornsak Faungnawakij

Abstract The increasing rate of oil and gas production has contributed in arelease of oil-in-water emulsion or mixtures to the environmentwhich has become a pressing issue. At the same time, pollutionof the toxic cigarette butt has also become the growing concern.This study explores utilization of cigarette butt waste as sourceof cellulose acetate-based (CA) polymer to develop phaseinverted membrane for treatment of oil/water emulsion andcompared with commercial polyvinylidene difluoride (PVDF) andpolysulfone (PSF). Results show that CA-based membrane fromwaste cigarette butt offers an eco-friendly material withoutcompromising the separation efficiency, with pore size rangesuitable for oil/water emulsion filtration with rejection of >94.0%.The CA membrane poses good structural property like that ofestablished PVDF and PSF membranes with equally asymmetricmorphology. It also poses hydrophilicity properties with contactangle of 74.5°, lower than both PVDF and PSF membranes. Thepore size of CA demonstrates the CA is within the microfiltrationrange with mean flow pore size of 0.17 µm. The developed CAmembrane shows a promising oil/water emulsion permeability of180 L m-2 h-1 bar-1 after five filtration cycles. However, it stillsuffers a high degree of irreversible fouling (>90.0%), suggestingpotential for future improvements. Overall, this studydemonstrates a sustainable approach in addressing issue ofoil/water emulsion pollution treated CA membrane from cigarettebutt waste.

The coverletter for this review report has been saved in thedatabase. You can safely close this window.

Authors' Responses to Reviewer's Comments (Reviewer 2)

Author'sNotes

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Author'sNotes File

Report Notes (/user/review/displayFile/17842024/DWAYc3EM?file=author-coverletter&report=11925660)

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Review Report Form

Englishlanguageand style

( ) Extensive editing of English language and style required ( ) Moderate English changes required ( ) English language and style are fine/minor spell checkrequired (x) I don't feel qualified to judge about the English languageand style

Yes Can beimproved

Must beimproved

Notapplicable

Does the introduction provide sufficient

background and include all relevant references?(x) ( ) ( ) ( )

Is the research design appropriate? ( ) (x) ( ) ( )

Are the methods adequately described? ( ) (x) ( ) ( )

Are the results clearly presented? ( ) (x) ( ) ( )

Are the conclusions supported by the results? (x) ( ) ( ) ( )

Commentsand

Suggestionsfor Authors

The work "Cigarette Butt Waste as Material for Phase InvertedMembrane Fabrication Used for Oil/Water Emulsion Separation"is interesting and useful for the research field.

Some requests and suggestions:

how many cigarettes have the cellulose acetate as butts?

how is reason to compare with the selected commercialmembranes?

figure 1 need consistency, and also f image is unclear!

a comparison with cellulose acetate membrane were welcome!

SubmissionDate

30 April 2021

Date of thisreview

04 May 2021 06:52:51

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Journal Polymers (https://www.mdpi.com/journal/polymers) (ISSN 2073-4360)

ManuscriptID

polymers-1223672

Type Article

Number ofPages

16

Title Cigarette Butt Waste as Material for Phase Inverted MembraneFabrication Used for Oil/Water Emulsion Separation

Authors Aris Doyan * , Chew Lee Leong , Muhammad Roil Bilad * , KikiAdi Kurnia , Susilawati Susilawati , Saiful Prayogi , ThanitpornNarkkun , Kajornsak Faungnawakij

Abstract The increasing rate of oil and gas production has contributed in arelease of oil-in-water emulsion or mixtures to the environmentwhich has become a pressing issue. At the same time, pollutionof the toxic cigarette butt has also become the growing concern.This study explores utilization of cigarette butt waste as sourceof cellulose acetate-based (CA) polymer to develop phaseinverted membrane for treatment of oil/water emulsion andcompared with commercial polyvinylidene difluoride (PVDF) andpolysulfone (PSF). Results show that CA-based membrane fromwaste cigarette butt offers an eco-friendly material withoutcompromising the separation efficiency, with pore size rangesuitable for oil/water emulsion filtration with rejection of >94.0%.The CA membrane poses good structural property like that ofestablished PVDF and PSF membranes with equally asymmetricmorphology. It also poses hydrophilicity properties with contactangle of 74.5°, lower than both PVDF and PSF membranes. Thepore size of CA demonstrates the CA is within the microfiltrationrange with mean flow pore size of 0.17 µm. The developed CAmembrane shows a promising oil/water emulsion permeability of180 L m-2 h-1 bar-1 after five filtration cycles. However, it stillsuffers a high degree of irreversible fouling (>90.0%), suggestingpotential for future improvements. Overall, this studydemonstrates a sustainable approach in addressing issue ofoil/water emulsion pollution treated CA membrane from cigarettebutt waste.

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Commentsand

Suggestionsfor Authors

The work "Cigarette Butt Waste as Material for Phase InvertedMembrane Fabrication Used for Oil/Water Emulsion Separation"in remake form should be published in POLYMERS journal.

The author responded to all suggestions and corrections whichwere recommended!

SubmissionDate

30 April 2021

Date of thisreview

18 May 2021 13:26:05